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Title: | 金屬沸石咪唑骨架材料衍生物應用於染料敏化太陽能電池及超級電容器 Zeolitic Imidazolate Framework-derived Composite Materials for Dye-sensitized Solar Cells and Supercapacitors |
Authors: | Siou-Ling Jian 簡秀玲 |
Advisor: | 何國川(Kuo-Chuan Ho) |
Keyword: | 硫化鈷,染料敏化太陽能電池,電觸媒,超級電容器,金屬沸石咪唑骨架,硒化鋅, cobalt sulfide,dye-sensitized solar cell,electrocatalyst,supercapacitor,zeolitic imidazolate framework,zinc selenide, |
Publication Year : | 2018 |
Degree: | 碩士 |
Abstract: | 本論文旨在研究金屬沸石咪唑骨架材料衍生物作為電極材料,用以發展低成本、高效能的能源領域(染料敏化太陽能電池和超級電容器)。本論文主要分為兩大部分:金屬沸石咪唑骨架衍生之硒化鋅摻雜氮碳材複合物作為對電極應用於染敏電池(第三章),和奈米碳管/金屬沸石咪唑骨架衍生之硫化鈷複合材料應用於超級電容器(第四章)。
在第三章中,以金屬沸石咪唑骨架衍生之硒化鋅摻雜氮碳材複合物作為染敏電池電催化材料,其表現出極佳的電催化特性和導電性。利用不同的碳化溫度及硒化溫度來合成金屬沸石咪唑骨架衍生複合材料,分別克服材料之導電性不佳的缺點和提升其電催化性。在此複合材料中,金屬沸石咪唑骨架碳化後之氮摻雜碳材有利於電催化及電子傳導;同時,鑲嵌在碳材中的硒化鋅則扮演加速催化三碘化物離子之活性催化點。最適化後之複合材料,其光電轉化效率為8.69%,高於傳統使用的鉑對電極(8.26%)。而在較弱光強度下,此複合材料仍有7.99%的光電轉換效率。此研究成果顯示此複合材料具有作為染敏電池之電觸媒的潛力。 在第四章中,合成了奈米碳管/金屬沸石咪唑骨架衍生之硫化鈷奈米複合材料作為超級電容器之電極材料。利用不同濃度的奈米碳管和金屬沸石咪唑骨架之前驅物合成不同粒徑大小的複合物。經過硫化過後,此奈米複合材料能同時具備高導電性及良好的電化學特性。此奈米複合材料中,奈米碳管扮演電子快速傳遞的通道,克服了硫化鈷導電性不佳的缺點。電化學實驗結果顯示,其可在5 A g-1的充放電電流密度下達到2173 F g-1的比電容值,同時在1000圈的充放電循環後,仍可維持91%的初始比電容值,顯示此奈米複合材料具有作為超級電容器之電極材料的潛力。 This thesis mainly focuses on two different but related parts, namely, discussing about the application of a zeolitic imidazolate framework-derived ZnSe/N-doped carbon cube hybrid electrocatalyst as the counter electrode for dye-sensitized solar cells (Chapter 3) and carbon nanotube/zeolitic imidazolate framework-derived cobalt sulfide hybrid composites for supercapacitors (Chapter 4). The overview of these two applications will be displayed in introduction (Chapter 1). Moreover, the experimental procedures (Chapter 2) includes the chemical reagent, material characterization and the principle of electrochemical analysis. In Chapter 3, a zinc selenide decorated N-doped carbonaceous hybrid material (ZIF-ZnSe-NC) derived from a zeolitic imidazolate framework (ZIF-7) used as the electrocatalyst for the counter electrode in DSSCs exhibited excellent electrocatalytic performance and electrical conductivity. Carbonization and selenization at different temperatures for synthesizing ZIF-ZnSe-NC electrocatalyst were carried out step by step to enhance the electrocatalytic performance and electrical conductivity of the material. In the ZIF-ZnSe-NC hybrid electrocatalyst, the N-doped carbon cube is beneficial to the electrocatalytic performance and the electrical conductivity. Meanwhile, embedded ZnSe in the carbon matrix also serves as the additional active site for facilitating I3- reduction. The DSSCs with the optimized ZIF-ZnSe-NC-11 wt% CEs exhibited a photovoltaic conversion efficiency (η) of 8.69 ± 0.13%, which is higher than that of the cells with Pt CEs (8.26 ± 0.02%). A reasonable cell efficiency of 7.99 ± 0.01% was still attained for the DSSCs with CEs of ZIF-ZnSe-NC-11 wt% at a dim light intensity of 10 mW cm-2. Thus, it could be concluded that the ZIF-ZnSe-NC is a promising material to replace the expensive Pt in DSSCs, especially for the indoor application. In Chapter 4, a hybrid structure of carbon nanotubes interconnected zeolitic imidazolate framework (ZIF) derived cobalt sulfide (CNT/CoS) nanocage was designed and synthesized as the electrode material in SCs. The carbon nanotubes/ZIF-67 (CNT/ZIF-67) nanocomposites with controlled ZIF-67 particle sizes have been systematically studied by varying the mass ratio of CNT to ZIF-67 under reaction process, then followed by subsequent sulfurization with thioacetamide. Benefiting from the porous nanocage architecture and conductive CNTs, the optimized CNT/CoS nanocage exhibits excellent electrochemical performance with an outstanding specific capacitance (2173.1 F g-1 at 5 A g-1), good rate capacity (65% retention at 20 A g-1), and long-term stability (91% retention over 1000 cycles), demonstrating a great potential in energy applications. The method developed in this work can be extended to the construction of other metal sulfide electrode materials for a variety of energy storage applications. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/76427 |
DOI: | 10.6342/NTU201801254 |
Fulltext Rights: | 同意授權(全球公開) |
metadata.dc.date.embargo-lift: | 2023-07-06 |
Appears in Collections: | 化學工程學系 |
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